Tin sulfide has outstanding thermoelectric properties in the b-axis direction of crystallography as a IV-VI group layered compound, which arouses great attention. In this study, temperature-dependent Raman spectroscopy (TDRS) is used to quantify the phonon anharmonicity in SnS crystals from 77 to 475 K, where the three-phonon process dominates in this temperature region. Moreover, integration of the four-phonon process and lattice thermal expansion will better describe the temperature-dependent Raman experimental phenomenon. The good agreement between the calculated and experimental lattice thermal conductivity confirms the three-phonon scattering process is the dominant scattering mechanism at this temperature range. Further, combining the atomic thermal displacement and charge density through density functional theory calculation, the inherently low thermal conductivity of SnS is because of strong lattice anharmonicity, which is brought by the presence of asymmetric chemical bonding resulting from the Sn 5s2 lone pair electrons. These results provide key insights for studying thermal properties of other low-dimensional materials.